Adhesively bonded CFRP/Al joints have been widely used in various engineering fields. However, the poor interface adhesion between the adhesive and the Al adherend limits its further use. In this study, ultrasonic vibration was applied to promote the interface adhesion, and the promotion mechanism was studied in detail. The vibration was exerted on the surface close to the bonding area after the adhesive was applied. According to the bonding strength test, this process improved the bonding strength and repeatability by approximately 32% and 48%, respectively. By comparing the failure behavior without and with ultrasound, it can be seen that ultrasound promotes interface adhesion of the adhesive/Al adherend significantly. Under the application of ultrasonic vibration, a tight microscopic bond was formed at the bonding interface, and a chemical reaction occurred to form chemical bonds. The opening of the epoxy group was promoted to allow Al to react with ?O?C to form Al?O?C, because attack of electrophilic Al?+?on O? of the epoxy group was strengthened by high-frequency impact between the adhesive and the Al adherend at the interface caused by the ultrasonic vibration. It can be seen that the application of ultrasonic vibration during the adhesive bonding process can promote interface adhesion between Al and the adhesive in terms of physics and chemistry, thus significantly improving the performance of the adhesive bond.